Lewis acid-mediated interfacial accelerated mass transport and electron transfer for enhanced oxygen reduction electrocatalysis

Single-atom catalysts are widely recognized as promising candidates in oxygen reduction reactions (ORR). However, achieving high activity remains challenging due to the limited interfacial reaction processes of key reactants and intermediates. Herein, we propose an optimization of Lewis acid-mediated interfacial processes to enhance the ORR performance of FePc. It was found that modifications in site acidity improved the interfacial water molecule network, thereby enhancing the transport of reactant oxygen and facilitating the subsequent protonation process. Additionally, the formation of the Fe–S Lewis pair effectively reduced the intermediate adsorption strength, which contributed to the improvement of high catalytic activity. This work not only highlights the crucial role of Lewis acid-base interactions in the ORR at the single-atom scale, but also provides a new avenue for the development of non-carbon-based single-atom catalysts in energy conversion and storage applications.